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The Diocese of Chatham was erected 8 May 1860, as the Diocese of Chatham, and covered the entire north of the Province of New Brunswick.

In its early years, Irish clergy dominated its affairs, though there was a French Catholic majority population in more northerly Restigouche and Gloucester Counties. Northumberland County, where Chatham was located, was predominantly Irish and Scottish Catholic. Over time, however, the tendency of the Irish to prefer an urban life, and move to Boston and other parts of the US, reduced the English-speaking Catholic populations, especially in the northern counties.

The first bishop was The Most Reverend James Rogers who retired in 1903, a well-respected and portly Irishman who did much to build the Catholic Church in the Diocese. Religious institutes were brought in, schools and hospitals built and vocations harvested. A fine cathedral, now St. Michael's Basilica was constructed, with a matching Bishop's Palace which housed the diocesan administration as well as the bishop. Colleges were opened in Chatham for the English (now St. Thomas University) and Bathurst for the French (Collège du Sacré-Coeur de Bathurst, merged into Université de Moncton). Bishop Thomas Barry continued Bishop Roger's work from 1902 to 1920.

The next appointment in 1920 was a French speaker. By this time the French were in a majority in the diocese, and Bishop Patrice Chiasson decided to move his headquarters to Bathurst, a majority French-speaking area. The move was complete in 1938 and it was renamed on 13 March 1938.

Bishop Camille Leblanc, who served from 1942 to 1969, was especially esteemed for his simplicity and frugal life style.